Researchers disentangle two competing mechanisms that govern how a promising semiconductor material responds to light
When light is absorbed by a semiconductor, it first creates an electron-hole pair before free charges can be generated. The electron and hole can remain bound together in a quasiparticle known as an exciton. This intermediate stage is important because excitons determine how light is absorbed and emitted, and how efficiently a material can convert light into electrical current.
Monolayer tungsten diselenide (WSe₂) is a material that researchers are investigating for use in photodetectors, optical computing and quantum technologies. It is an atom-thick semiconductor that interacts very strongly with light. The excitons formed in WSe₂ are unusually stable, allowing quantum effects to be observed particularly strongly. WSe₂ therefore provides a model system for learning how to control light-generated excitons, knowledge that could eventually lead to more efficient solar cells, photodetectors and low-energy photonic technologies.
A key question in this area of research is what causes the WSe₂ exciton energy to shift to a higher energy (blue shift), a lower energy (red shift) or split into two levels. Two leading explanations are the Optical Stark Effect, in which the laser’s electric field directly modifies the exciton energy, and exciton-exciton interactions, in which excitons alter one another’s energies through many-body interactions.
In this work, the researchers used helicity-resolved transient absorption spectroscopy to show that, while the laser pulse is present, the Optical Stark Effect dominates, causing a blue shift, splitting or a red shift depending on the laser detuning. After the pulse ends, exciton-exciton interactions become dominant, producing a blue shift. By varying the laser detuning and tracking the exciton response on femtosecond timescales, the researchers were able to separate the coherent Optical Stark Effect from the later incoherent exciton-exciton interaction. The work provides a clearer picture of how light and excitons interact on ultrafast timescales, which is important for the design of next-generation optoelectronic devices.
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Intercalation in two-dimensional transition metal chalcogenides: interlayer engineering and applications by Dibyendu Ghosh, Pooja Devi and Praveen Kumar (2022)
